Spheroidal crystal sugar and method of making

ABSTRACT

The present invention is a new spheroidal polycrystallite product and a process for making the same. In the present invention amorphous sugar is transformed to crystalline sugar by hydrating rather than dehydrating sugar. The product of the present invention is unique in shape, size, and possesses a high degree of uniformity.

BACKGROUND OF THE INVENTION

The present invention relates to crystalline sugar products, and, inparticular, to a new form of crystalline sugar.

Crystallization is one of the oldest industrial chemical transformationprocesses known. Vast quantities of crystalline substances are producedfor commercial purposes, e.g., in excess of 100×10⁶ metric tons peryear. One of the most common products prepared by crystallization issugar.

Crystallization of sugar is complex. The growth of crystals involvessimultaneous transfer of heat and mass in a multi-phase, multi-componentsystem. While the co-existence of these conditions alone present complexcontrol problems, fluid and particle mechanics and thermodynamicinstability create further complications.

Conventional wisdom in the science of sugars teaches crystallization bysupersaturation. Supersaturation requires removal of water. Cooling,evaporating, and precipitating are used. Manufacturing procedures forcrystallizing sugar are heat and energy intensive. Moreover, nucleationof sugar crystals during supersaturation is relatively uncontrollable.Consequently, the size and shape of the resulting crystals areunpredictable.

The drawbacks of known sugar manufacturing procedures are especiallymanifested when preparing sugar having reduced-size crystals.Reduced-size crystalline sugar product is referred to herein asmicrocrystals. Individual particles of microcrystalline product are nogreater than 50 μm.

Classification of crystallizers known in the industry follows themethods by which supersaturation is achieved. The technical aspects ofprocedures used for sugar crystallization are well documented, and theyare generally high-energy procedures.

For example, one method of manufacturing reduced-size crystals involvesgrinding and sieving crystalline sugar. Grinding is energy intensive.Moreover, fracturing sugar results in a wide distribution of groundsugar crystals. The large crystals must be reground and sieved. Much ofthe product is lost as fines. Thus, grinding and sieving is expensiveand inefficient.

U.S. Pat. No. 3,981,739 to Dmitrovsky, et al. discloses preparation ofcrystalline sugar from solution by 1) concentrating a solute in thepresence of seed crystals added thereto, followed by 2) further removalof solvent through heating and evaporation of the stream resulting fromthe first stage concentration. This energy intensive procedure producessugar crystals having an average size in the range of 325-425 microns.The Dmitrovsky, et al. '739 disclosure is a solution process whichrelies on nucleation by addition of seed crystals while concentrating byhigh heat and vacuum evaporation. The same procedure is disclosed inU.S. Pat. No. 4,056,364 to Dmitrovsky, et al.

U.S. Pat. No. 4,159,210 to Chen, et al. describes a method for preparingcrystallized maple sugar product by 1) concentrating maple syrup to asolids content of about 93-98% in the presence of heat and partialvacuum, and 2) impact heating until transformation and crystallizationof the syrup occur. The product may then be cooled, milled and screenedto a suitable size range. The Chen, et al. '210 procedure is energyintensive, relies on "beating" to induce nucleation of the crystals, andcalls for subsequent milling to obtain reduced-size crystals.

In U.S. Pat. No. 4,362,757 to Chen, et al. a crystallized sugar productand a method of preparing same are described. The method disclosed inthe Chen, et al. '757 reference includes concentrating sugar syrups to asolids content of about 95% to about 98% by heating to a temperature ofabout 255° F. to about 300° F. The resulting concentrated syrup ismaintained at a temperature not less than about 240° F. in order toprevent premature crystallization. A premix consisting of an activeingredient (e.g., a volatile flavor, an enzyme, an acidic substance suchas ascorbic acid, a fruit juice concentrate, or a high invert sugarsubstance) is mixed with the concentrated sugar syrup. The combinationis subjected to impact heating until a crystallized sugar product madeup of fondant-size sucrose crystals and the active ingredient is formedwhich has a moisture content of less than 2.5% by weight. The Chen, etal. '757 process requires heat intensive concentrating and heating fornucleation.

A similar procedure is disclosed in U.S. Pat. No. 4,338,350 to Chen, etal. wherein a process for preparing a crystallized sugar productcontaining a food ingredient is described. The Chen, et al. '350disclosure calls for concentrating a sugar syrup at a temperature rangeof about 250° F. to about 300° F. to a solids content of about 90 to 98%by weight. A food ingredient, such as gelatin, cocoa powder, pectinconcentrate, etc., is admixed with the sugar syrup. The mixture issubjected to impact beating until a crystallized sugar product made upof aggregates of fondant-size sucrose crystals and food ingredients isformed. The Chen, et al. '350 process requires heat intensiveconcentrating and beating to induce crystallization.

U.S. Pat. No. 3,365,331 to Miller, U.S. Pat. No. 4,338,350 and U.S. Pat.No. 4,362,757 describe a process for crystallizing sugar, which involvesimpact beating a sugar solution to provide nucleation. The processinvolves input of considerable amount of energy and has problemsdirectly related to temperature control.

Other disclosures include British Patent Specification No. 1 460 614 andU.S. Pat. No. 3,972,725 (Tate & Lyle Limited) which disclose acontinuous process wherein a syrup solution is catastrophicallynucleated and discharged into a crystallization zone. Catastrophicnucleation is achieved by subjecting the solution to shear force whichcan be applied in apparatus such as a colloid mill or homogenizer. Thesolution is discharged onto a moving band where the water must be boiledoff by maintaining the material at a relatively high temperature. Arelated process has been disclosed in British Patent Specification 2 070015 B and U.S. Pat. No. 4,342,603, which is used for crystallization ofglucose. In the disclosed procedure, a supersaturated solution issubjected to shear force and allowed to crystallize on a belt. Both thesucrose process and the glucose process require solution processing athigh temperatures and are, consequently, energy intensive.

U.S. Pat. No. 3,197,338 to Hurst, et al. discloses a process forcrystallizing glucose which includes kneading a glucose solution toinduce nucleation followed by crystallization to form a solid glasswhich is then ground. Another glucose crystallization process has beendisclosed in GB 2 077 270 B in which starch hydrolyzate is concentratedby evaporation and then simultaneously crushed and mixed duringcrystallization while cooling. The product is further milled. Theseprocesses also require nucleating by beating a solution which includesglucose.

UK Patent Specification G B 2 155 934 B of Shukla, et al. discloses amethod for crystallizing sucrose or glucose from a solution. Shukla, etal. subject a sugar solution to evaporation to produce a supersaturatedsugar solution. The supersaturated solution is then subjected to shearin a continuous screw extruder to induce nucleation. The retention timeof the syrup is below 25 seconds (on the average) at a temperature of115° C. to 145° C. (239° F.-293° F.) for sucrose and 100° C.-135° C.(215° F.-275° F.) for glucose. After the syrup is subjected toprogressive nucleation, Shukla, et al. pass the syrup onto a moving bandto permit crystallization to continue at a gradual rate at relativelyhigh temperature. The Shukla, et al. process requires maintenance of thesolution at temperatures which do not drop below the boiling point ofwater.

Additional technology has been developed which relates to processingfood and food ingredients. For example, a series of U.S. patents issuedto Thomas E. Chivers (U.S. Pat. No. 3,762,846, U.S. Pat. No. 3,723,134,and U.S. Pat. No. 3,557,717) disclose a solution process for makingcandy floss from a cooked slurry or syrup. The ingredients are blendedand heated at a first temperature, e.g., 200°-205° F. (93°-96° C.), toform a slurry. After forming the slurry, the batch is cooked or boiledat a substantially higher temperature, e.g., about 340° F. (171.1° C.),and thereafter discharged through an atomizing nozzle. Most of themoisture contained in the molten candy flashes off as it is discharged.The Chivers disclosures rely on dissolution of the ingredients, e.g.,sugar and other ingredients, in water and then heating extensively todrive the water from the solution. Most of the water is driven off afterdischarging the solution. Thus, the Chivers technology suffers fromdrawbacks associated with sustained high temperature processing anddissolution of ingredients during processing.

Another method for processing material is disclosed in European PatentApplication 0 387 950 A1 of Stork. The Stork process is a method ofpreparing a foam spray-dried product by collision of a stream of gaswhich contains dry particulate material, with a jet of droplets of aliquid solution. A liquid solution which contains at least one of theingredients of the end product is combined with gas and heated beforespraying as a jet of droplets for collision with the dry particulate.The Stork system is designed to process a low density product; itrequires an elaborate equipment arrangement, and is energy intensive.

In U.S. Pat. No. 3,615,671 to Shoaf discloses a method of producing foodproducts by encasing dry particulate food particles within a casing ofspun sugar filaments. In order to enhance 1) shaping of the fibers andparticles and 2) the tendency of the fibers to stick to each other witha minimum of compression, Shoaf uses a humectant in the sugar mix to bespun and controls the relative humidity of the gases surrounding thefilaments as they are spun. The humectants described as useful are asfollows: invert syrup or corn syrups and polyhydric alcohols, e.g.,sorbitol, glycerol and pentahydric alcohols, e.g., xylitol. Shoaf isconcerned with preventing crystallization of the spun sugar in order toenable the manufacturer to encase dry food particles by wrapping andcompressing filaments of the spun sugar around the particles.

More recently, a trade brochure provided by Domino Sugar Corporation,Industrial Products, entitled "Co-Crystallization" (undated) describes aproduct in which microsized crystals form aggregates having a secondingredient disposed over the surface of each aggregate. The process forproducing this new product requires that all starting materials must bein a liquid state. Therefore, solvent must be driven off by heat and/orvacuum in order to concentrate the syrup for crystalline growth. As inother solution process energy is required to transform the sugar tomicrosized crystals.

Inherent in the procedures set forth above, as well as other proceduresknown in the art, is the technical philosophy of dehydration to promotecrystallization. Supersaturation, pan drying, and nucleation byagitation or chemical reaction depend on the principle of eliminatingwater to form crystals. A common difficulty with crystallization basedon this technical underpinning has been lack of control over crystallinegrowth.

Thus, it would be significant advance in the art of crystallization, toprovide a mechanism for crystal formation which departs from traditionaldehydration, and which provide a low energy means for producing acrystalline sugar product.

Accordingly, it is an object of the present invention to enable theartisan to make a sugar product which has a predictable and uniformcrystal size without energy-intensive procedures. Other objects andsurprising new sugar-crystal technology are disclosed in the remainderof the Specification.

SUMMARY OF THE INVENTION

The present invention is a new form of crystalline sugar as well as amethod of making same. The new crystalline sugar consists ofsubstantially spheroidal polycrystallite structures. The polycrystallitestructures, in turn, are made of sugar crystallites which are quitesmall, i.e., on the order of less than 10 μm, and are quite uniform insize. In fact, the spheroidal polycrystallite structures can bemonodispersed, and the crystallites themselves are monodispersed asdefined hereinbelow. In a preferred embodiment of the present invention,the spheroidal polycrystallite structures are microcrystalline, i.e.,have a greatest dimension of not more than about 50 μm.

Contrary to the teachings in the art of sugar crystallization, the newsugar product is prepared in accordance with the present invention byadding water to amorphous sugar. Amorphous sugar as used herein means asugar stock which contain a high percentage of amorphism, i.e., greaterthan 50% by weight, and preferably greater than 70% by weight of thesugar stock is amorphous. The unique procedure of this inventionincludes contacting amorphous sugar with a non-aqueoussugar-nondissoluble liquid and water so that the water is made availableto the amorphous sugar at a controlled rate and in an amount whichpermits growth of the spheroidal polycrystallite structures.

While the present invention primarily concerns sugars as defined herein,it is also intended to include processing (and products therefrom) anyamorphous solid form of a solvent-soluble compound which is capable offorming crystals. Such compounds may include lactose, polydextrose,maltodextrins, etc. Preferably the solvent for the process andproduct(s) herein is water.

Amorphous sugar can be provided by shearform processing asugar-containing feedstock. A shearform process according to the presentinvention is one in which a feedstock is subjected to shear and heatsimultaneously in order to obtain flash flow. One shearform processincludes subjecting a feedstock containing sugar to shear created byhigh speed spinning on a spinning head. The spinning head casts thematerial outwardly as the feedstock undergoes flash flow. Flash flow iscreated as a consequence of the simultaneous application of heat andshear. An alternative shearform process includes heating anon-solubilized feedstock having a sugar carrier sufficiently to provideinternal flow. The feedstock is ejected while the sugar possessesinternal flow, and is then subjected to disruptive fluid shear force toform multiple masses of carrier. Other methods are contemplated whichprovide the same critical conditions of heat and shear so that asubstantially solid feedstock which contains sugar can be transformedphysically and/or chemically from a solid structure to an essentiallyamorphous solid structure.

An additive can be included in the amorphous sugar and become part ofthe resulting polycrystallite structures and the crystallitesthemselves. This is referred to herein as co-crystallization. When suchan additive is provided, it is included without reducing the amorphismof the sugar and without deteriorating the resulting polycrystallitestructures. Additives contemplated for use herein, include, but are notlimited to, flavorants, bio-affecting agents, dyes, fragrances, foodproducts, food ingredients, and other compatible agents. Flavorants inthe present invention includes sweeteners of all types, natural andsynthetic.

In a further embodiment of the present invention, co-crystallization canbe effected by using an additive, especially a bio-affecting agent, as anucleating agent. This is another mode of co-crystallizing because thenonsugar additive is introduced during crystallization--not duringformation of amorphous sugar. The bio-affecting agent is made availablein the solvent (e.g., water) which is used to initiate and promulgategrowth of sugar crystals from amorphous sugar. Consequently, thebio-affecting agent actually serves as a nucleating agent.

A non-aqueous sugar-nondissoluble liquid means a liquid which containssubstantially no water and in which sugar does not dissolve, i.e., lessthan 1 gr. of sugar will dissolve in 50 ml of the liquid. One suchliquid is ethanol. The non-aqueous sugar-nondissoluble liquid can alsobe a blend of two or more nonsolvents.

In a preferred embodiment of the present invention, the non-aqueoussugar non-dissoluble liquid and water form an azeotrope, and, in themost preferred embodiment of the present invention, the water and theliquid are combined within an azeotropic range. An azeotropic mixture isa mixture wherein distillates of the mixture have the same compositionof components as does the liquid mixture. Thus, in the case of water andanother liquid medium, the mixture will distil at the same ratio ofcomponents which are present in the mixture.

The present invention involves the use of ambient systems which includea nondissoluble liquid and a solvent component. In all cases herein thecomponents possess their salient characteristics, i.e., nondissolubilityand solvent characteristics, at room temperature, e.g., 28°-32° C.

Water is provided in the non-aqueous sugar-nondissoluble liquid in anamount sufficient to enable the amorphous sugar to be controllablycrystallized to form spheroidal polycrystallite structures. It has beenfound in the preferred mode that water is present in an amount notgreater that about 5%, and preferably not greater than about 2%.

Other effects can be achieved by including a surfactant in the feedstockwhich is used to make the amorphous sugar. By using a surfactant, auniform tiny crystal product can be made with a high degree ofpredictability. Lecithin has been found to be the preferred surfactantat this time. It is expected that other surface active agents will beidentified which enhances the procedure and product of the presentinvention, and it is intended to include such additional surface activeagents within the scope of the claimed invention.

In order to obtain as a separate product the crystallites which combineto form the polycrystallite structure, the spheroidal polycrystallitesare disintegrated. This has been achieved by contacting the spheroidalpolycrystallite structures with a sugar-saturated liquid, e.g., greaterthan about 67% sugar (sucrose). The resulting crystallites are highlyuniform, i.e., monodispersed, and have a very tiny size, i.e., on theorder of about 5 μm.

A further manifestation of the present invention is a comestiblecomposition which can be used as a coating or filler for baked goods.Coatings and fillers as used herein means a non-baked portion of anedible product, such as cookie fillings, cake fillings (e.g., Twinkie™fillings, etc.) icings, and other coatings. These coatings and fillingsinclude either the spheroidal polycrystallites or crystallites or both,and other ingredients which preserve organoleptic properties, e.g.,texture, moisture level, prevention of crystallization, et al.Additional ingredients employed to achieve the preservation of thecoatings and fillers include, but are not limited to, gums, humectants,fats, and flavors (including sweeteners). The present invention includesthese compositions.

As a result of the present invention an entirely new crystalline formhas been provided. This crystalline form has been found to be extremelyuseful in products which require a uniform crystal sugar product. Forexample, a new fondant consisting of substantially spheroidalpolycrystallite structures can be prepared. In yet a further preferredembodiment, a fondant product can be prepared which uses monodispersedsugar crystallites. The resulting product is amazingly smooth andflowable, and has an entirely different microscopic composition from anyknown fondant product.

One of the distinct advantages of the present invention is that the sizerange of the product can be selected for the intended use. Moreover, thenature of the process of the present invention enables the artisan tomake a crystalline product of a particular size and shape with a veryhigh degree of predictability. Reduced-size crystals can be efficientlyproduced without the use of energy-intensive grinding and sieving. Thisis a significant departure from crystalline products and processes ofthe past.

As a result of the present invention a new fat mimetic ingredient isprovided for use in foods, e.g., fondants, frosting, fillers for bakedgoods--especially cookie fillers, etc.

Moreover, an extremely efficient tableting vehicle is provided. Activeagent can be incorporated into the crystalline product, and thecrystalline product, (with or without active agent), can be used as anexcipient.

The present invention has uniquely harnessed the natural drive of matterto seek and maintain a lower energy state, to create a process forcontrolled crystalline growth as well as new product resultingtherefrom. Material which has a natural crystalline structure in itslowest entropy state is transformed to an increased entropy state whenit is made amorphous. In the amorphous condition the material possessesa natural tendency to attain a lower energy state--i.e., the crystallineform of the material. The inventors herein have harnessed this naturaltendency of matter to drive controlled crystallization. This has beenachieved by providing an essentially non-solvent system in which acontrolled amount of solvent (for the particular matter) is madeavailable to permit controlled crystallization. The variety ofprocedures and products resulting from harnessing of nature's tendencyto seek its lowest entropy state are boundless, and the present claimscover any procedure which utilizes the principles set forth herein.

For a better understanding of the present invention, reference is madeto the Drawings, the following Detailed Description and non-limitingexamples. The scope of the invention is described in the claims whichfollow the detailed description.

BRIEF DESCRIPTION OF THE DRAWINGS

FIG. 1 is a detailed photomicrograph of the unique spheroidalpolycrystallite of the present invention;

FIG. 2 is a schematic representation of the polycrystallite structure ofthe present invention in partial cross-section;

FIG. 3 is a graphical representation of the results of experimentsconducted to determine the effect of percentage of water content innon-aqueous sugar-nondissoluble liquid;

FIG. 4 is a graphical representation of the effects of residence time ofamorphous sugar in non-aqueous sugar-nondissoluble liquid at less than1.0% water content; and

FIG. 5a and 5b are photomicrographs which compare the uniquecrystallites produced in accordance with the present invention tofondant crystals available from processes known in the art.

DETAILED DESCRIPTION OF THE INVENTION

The present invention is a new crystalline sugar in the form of asubstantially spheroidal polycrystallite structure. See FIG. 1 which isa photomicrograph of spheroidal polycrystallites produced in accordancewith the present invention shown at 3.0K magnification. By substantiallyspheroidal is meant that the structure is formed with a sphericalcenter. However, the final crystalline product can also assume the shapeof a dome or a raspberry-like structure. Many of the structures will becompletely spheroidal. In any event, substantially spheroidal isintended to include all such polycrystallite structures which possess aspheroidal center.

The term polycrystallite, is meant to describe the spheroids as beingcomposed of many tiny crystallites. The spheroidal polycrystallites ofthe present invention have at least 20, but preferably more,crystallites arranged around a spheroidal center. In fact, uponmicroscopic inspection of the structures, one can detect the individualtiny crystallites arranged as a "coat of mail" about a spherical center.See FIG. 1. These crystallites are on the order of several angstroms,i.e., less than 10 μm, and preferably less than 5 μm. Thepolycrystallite spheroids can be disintegrated to release thecrystallites. For example, crystallites can be released by contact witha saturated sugar solution. In a preferred embodiment, the spheroidalpolycrystallites of the present invention can be determined byidentifying at least 20 crystallites while dissolving the spheroids witha saturated sugar solution. This crystallite product has been found tobe ideal for formation of a fondant, e.g., cake icing, confectioneryfillings, coated candy fondants (such as chocolate coated), etc. Theproperties of the polycrystallite sugar product make it ideal to replaceall (or some portion) of the fat in comestibles such as frostings,fillings, etc. The organoleptic sensations created by fat are closelyemulated or replaced by use of the present product.

The spheroidal polycrystallites of the present invention have a trulyunique capability of building the viscosity of a fondant composition ata relatively low sugar concentration. A fondant is a soft, creamy candymade of sugar, and is normally used as a filling for other candies. Forexample, if it is normally necessary to include 67% by weight ofcommercially-available fondant sugar to achieve the correct viscosity ina fondant, only about 37% by weight (or about 1/2 the amount of thecommercial fondant sugar) of the polycrystallite sugar is required toachieve the same. This is a truly remarkable effect which is furtherdescribed in the examples.

Another unique feature of a preferred embodiment of the presentinvention is that the spheroidal polycrystallite structures can bemonodispersed. Monodispersion of spheroidal polycrystallites meansnon-agglomerated polycrystallites. Even the crystallites themselves aremonodispersed. Monodispersed as used herein refers to the production ofa highly uniform crystalline product. As previously explained,crystalline sugar prepared by methods known in the art result in a widevariety of crystal sizes. This is due to many factors, all of whichcontribute to the basic lack of control over the nucleation and growthof crystals. In the present invention, however, the new spheroidalpolycrystallite structures are grown to a predictably uniform size.

"Monodispersed" as used herein means that at least about 60% by weight,preferably at least 80% and most preferably at least 90%, of thecrystals have a largest diameter which is within 60% of the mean crystaldiameter. Crystal diameter is that dimension which is the greateststraight line dimension in the largest plane taken through a threedimensional crystal.

Referring to FIG. 2, if one considers a crystal C which has threedimensions in the x, y, and z directions, the crystal diameter is thegreatest straight line dimension L in the largest plane P through thecrystal.

In yet a further preferred embodiment mono-dispersibility means that atleast 60% of the crystals are within 50% of the mean crystal diameter,and in a most preferred embodiment within 40% of the mean crystaldiameter.

In view of the fact that such a significant percentage of the crystalscan be grown to within a very uniform size range, significant advantagesare obtained in the use of the product.

The process of the present invention is quite unique in that it employsa procedure which is directly opposite the classic teaching of the sugartechnology to form a crystal by concentration and/or supersaturatingsugar from a solution. In fact, the present invention employs aprocedure which requires controlled addition of a sugar solvent,preferably water. Water is controllably added to form the uniquecrystals and promote unique crystalline growth claimed herein.

In the preferred embodiment of the present invention, the amorphoussugar is provided by shearform processing a sugar-containing feedstock.In the present invention, amorphous sugar is formed from "sugars.""Sugars" are those substances which are based on simple crystallinemono- and di-saccharide structures, i.e., based on C₅ and C₆ sugarstructures. "Sugars" include sucrose, fructose, lactose, maltose, andsugar alcohols such as sorbitol, mannitol, maltitol, etc. The sugar ofchoice in the present invention is sucrose.

A shearform sugar product is a substantially amorphous sugar whichresults from subjecting sugar to heat and shear sufficient to transformcrystalline sugar to amorphous sugar without the use of a solution.Thus, in the sense of the present invention, a shearform sugar productis characterized as a sugar product resulting from a non-solubilizedsugar. It can be the starting material for forming the uniquecrystalline product of the present invention. However, any amorphoussugar can be used.

This entire concept is directly contrary to the prior art whichspecifically teaches the artisan to crystallize sugar by eliminating ordehydrating solvent by driving it off with heat and/or vacuum.

A further aspect of the present invention is co-crystallization. Anycompatible additive can be included internally in the crystallite orpolycrystallite structures of the present invention so that the endproduct includes the additive(s). Such additives can be selected fromthe group consisting of flavorants, bio-affecting agents, dyes,fragrances, food products, food ingredients, and other agents which arecompatible. Compatible means the additives can be included in theamorphous sugar without destruction of the amorphism, and can beincluded in the crystallite and polycrystallite structures withoutdeterioration thereof.

A non-limiting list of bio-affecting agents is as follows: antitussives,antihistamines, decongestants, alkaloids, mineral supplements,laxatives, vitamins, antacids, ion exchange resins,anti-cholesterolemics, anti-lipid agents, antiarrhythmics, antipyretics,analgesics, appetite suppressants, expectorants, anti-anxiety agents,anti-ulcer agents, anti-inflammatory substances, coronary dilators,cerebral dilators, peripheral vasodilators, anti-infectives,physcho-tropics, antimanics, stimulants, gastrointestinal agents,sedatives, antidiarrheal preparations, anti-anginal drugs,vasodialators, anti-hypertensive drugs, vasoconstrictors, migrainetreatments, antibiotics, tranquilizers, anti-phsychotics, antitumordrugs, anticoagulants, antithrombotic drugs, hypnotics, anti-emetics,anti-nauseants, anti-convulsants, neuromuscular drugs, hyper- andhypoglycemic agents, thyroid and antithyroid preparations, diuretics,antispasmodics, uterine relaxants, mineral and nutritional additives,antiobesity drugs, anabolic drugs, erythropoietic drugs, antiasthmatics,cough suppressants, mucolytics, anti-uricemic drugs and mixturesthereof.

The present invention is particularly useful in providing a new deliverysystem for inhalants. Inhalants must be formed of minute particles whichare rapidly absorbed by the patient. Thus, since sugar is quicklydissolved at body temperature, inhalants co-crystallized with the uniquetiny highly-uniform product of the present invention can be easilydelivered as a tiny particulate which is rapidly absorbed by the body.

Any amorphous sugar can be used, but the present preferred embodimentsinclude the use of amorphous shearform product. The shearform product ofthe present invention can be made on machines such as those used formaking cotton candy. In these machines, sugar is introduced to a spinnerhead in which it is subjected to heat and shear created by centrifugalforce from the spinning head. Disclosures which relate to spinningsubstances include U.S. Pat. Nos. 4,855,326, 4,873,085, 5,034,421,4,997,856, and 5,028,632.

Examples in the U.S Patents listed above describe processing feedstockmaterial by subjecting it to high speed spinning on a spinning head inwhich the substance is also subjected to heating by a heating element.The change of temperatures is quite large, which is believed to beoccasioned by the spinning head quickly and efficiently spreading thefeedstock material against the heating element circumferentiallydisposed around the perimeter of the spinning head. Thus, extensivesurface contact of the feedstock against the heating element isprovided. An additive can be included in the feedstock so thatco-crystallization results when processed according to the presentinvention.

More recently, commonly owned co-pending application entitled "Processfor Making Shearform Matrix," filed on Oct. 23, 1992 and assigned U.S.application Ser. No. 965,804, discloses another process for makingshearform matrix by subjecting non-solubilized feedstock to heatsufficient to induce internal flow, ejecting a stream of the feedstockwhile possessing internal flow, and then subjecting it to disruptivefluid shear force which separates it into separate parts or masseshaving a transformed morphology. The product is amorphous. Otheringredients can be included in the material so that when it is used inthe present invention, co-crystallization will occur.

The amorphous sugar, with or without the additive, is then contactedwith a non-aqueous sugar-nondissoluble liquid, and water. The purpose ofcontacting amorphous sugar with water in the environment of thenon-aqueous sugar-nondissoluble liquid is to achieve highly controlledcontact of the amorphous sugar with moisture. In this way the uniquespheroidal polycrystallite structures can be formed. In a preferredembodiment, the non-aqueous sugar-nondissoluble liquid is one whichcombines with water to form an azeotrope. An azeotrope is a liquidmixture which produces distillates having the same composition as theliquid mixture. A preferred non-aqueous sugar-nondissoluble liquid usedin the present invention is ethanol. Ethanol forms an azeotropic mixturewith water. It is believed that the affinity of ethanol to form arelatively inseparable combination with water enhances the controlexerted over the contact of water with the amorphous sugar. In anyevent, the water is presented to the amorphous sugar at a rate and in anamount which permits the spheroidal polycrystallite growth.

Generally, water is made available in ethanol by providing a 5% water inethanol mixture and preferably less than 1% water, at a temperature ofabout -10° C. to about 40° C.

As yet a further modification to the present invention, a surfactant canbe included in the feedstock which forms the amorphous sugar. The use ofa surface active agent in the feedstock enables the practitioner toexercise even greater control over crystal formation. It has been foundthat greater uniformity of crystal size is achieved. Furthermore,formation of aggregates is prevented by use of a surfactant. Finally,greater control of the size of the crystalline spheroids is alsoachieved. The preferred surfactant is presently lecithin. Lecithin canbe included in the feedstock in an amount of from about 0.1% to about5.0% by weight.

A further aspect of the present invention is a composition which includeeither the spheroidal polycrystallites or the crystallites or acombination of both, and which are used as fillings and/or coatings forbaked goods. These ingredients, which generally preserve theorganoleptic properties of the compositions, can include gums,humectants, fats, and flavors (including sweeteners). Other ingredientsmay be used, and the present invention is intended to include all suchcompositions which incorporate spheroidal polycrystallites and/orcrystallites.

Gums are generally considered carbohydrate polymers of high molecularweight, and include both natural gums and mucilages such as acacia,agar, alginic acid, carrageenan, guar gum, guaiac gum, karaya gum,tragacanth gum, xanthan gum, locust bean gum, and alginates, e.g.,calcium alginate, potassium alginate, and sodium alginate. Gums alsorefer to cellulosic gums which include hydroxypropyl methylcellulose,hydroxyethyl cellulose, methyl cellulose, carboxymethyl cellulose andhydroxymethyl cellulose.

Humectants are considered those agents which retain or help to retainmoisture in foods and include glycerine, potassium polymetaphosphate,propylene glycol, polyethylene glycol, sodium chloride, sorbitol, invertsugar and glycerol triacetate (triacetin), corn syrup and corn syrupsolids.

Fats are another class of ingredients which can be used in thecompositions of the present invention and generally include mono-, di-,and tri- glyceryl esters of higher chain fatty acids, e.g., stearic andpalmitic, or mixtures thereof, and can be solid or liquid. Fats can bederived from plants or animals.

With respect to flavors, the compositions of the present inventioninclude but are not limited to, flavors such as spices, acid flavors,sweeteners both synthetic and natural. Spice oleoresins are included inthe compositions of the present inventions.

EXAMPLES

In the following examples, amorphous sugar has been provided by spinningsucrose in a spinning machine operated at about 160° C. and spun at arate of about 3600 rpm. The product was in the form of a sugar floss.

ETHANOL EXAMPLES

Granulated sucrose was processed in a spinning device as set forthherein above to produce an amorphous fibrous cotton structure (floss).The volume of the floss was reduced by subjecting it to processing in ahigh speed mixer to break the fibers into smaller pieces.

Non-aqueous sugar-nondissoluble liquid was provided in the form ofanhydrous ethanol, i.e., 200 proof ethanol. Water was carefullyintroduced to the ethanol to create 11 different compositions ranging inwater content from 0.08 to 4.8% on weight basis. The compositions havebeen set forth below in an Ethanol/Water Table.

    ______________________________________                                        WATER/ETHANOL TABLE                                                           Water % in Ethanol vs. Particle Size                                          Particle Size (Microns)                                                       Water %          10%.sup.1                                                                            50%.sup.1                                             ______________________________________                                        .08              7.73   22.98                                                 0.62             9.34   24.26                                                 1.02             8.51   22.43                                                 1.53             11.35  30.43                                                 1.97             12.58  29.60                                                 2.44             18.84  42.70                                                 2.90             19.05  37.96                                                 3.17             16.54  34.19                                                 3.72             20.94  43.10                                                 4.14             20.89  40.26                                                 4.80             20.56  43.64                                                 ______________________________________                                         .sup.1 Average of three measurements                                     

A 2.5 gram sample of floss was added to 35 grams of each of theanhydrous ethanol/water compositions. Each mixture was stirred for about1 minute and then vacuum filtered to remove the ethanol and recovercrystal samples. The total contact time was about two (2) minutes.

Photomicrographs of the crystals were made which show the uniquespheroidal polycrystallite structure. The crystals resulting from theprocedure set forth above are depicted in FIG. 1.

Each of the crystal samples were analyzed in a Microtrac FRA particlesize analyzer. The analysis was conducted by three scans of 15 secondseach and average values were recorded. The results are reported in theWater/Ethanol Table and depicted in FIG. 3. The predominant particlesize was measured as a percentage of particles below a certain size.These sizes are entered in the table and on the graph in FIG. 3 as afunction of the ethanol/water composition in which they were produced.The results show that crystals produced by any given ethanol/watercomposition had 50% of its particles below a certain particle size,while 10% of the crystals were below a smaller size.

The results are consistent. They show that an increase in percent ofwater corresponds to an increase in the size of the crystals whichresulted therefrom. Thus, for example, 50% of the crystals grown at0.08% water content were below a particle micron size of about 23 μm,while 10% had a particle micron size below 8 μm.

Further experiments were conducted in which crystal growth was measuredas a function of contact time with anhydrous ethanol and less than 1.0%water. Referring now to FIG. 4, the crystal size has been depicted as itcorresponds to the time of exposure to the ethanol/water composition.One can see that after 5 minutes 90% of the particles had a size ofabout 68 μm or less, 50% of the particles were of a particle size ofabout 38 μm or less, and 10% of the crystal had a size of about 18 μm orless. The graph of FIG. 4 shows that up to sixty (60) minutes of contacttime resulted in little change in crystal size at the 50% range.

The results of the ethanol/water experiments show unique spheroidalpolycrystallite structure. The crystals are spheroidal in size and shape(e.g., dome, raspberry-like, etc.). Moreover, the results of the aboveexperiments show that the crystal sizes are highly uniform, i.e.,monodispersed.

Furthermore, the crystals can be very quickly produced, i.e., within 30seconds for the smaller size crystals. This is a significant departurefrom procedures known in the art which require high energy-consumingsteps such as heat-intensive drying and application of vacuum to removequantities of solvent, usually water, from a solution of sugar.

Moreover, the ethanol used in each of the crystallizations can berecovered and recycled for use again at the desired water content range.For example, the ethanol used in several of the experiments set forthabove was recycled after filtration and analyzed after the first, fifthand tenth runs. The results of these tests show that after the firstrun, the ethanol contained 0.82% water; after the fifth run, the ethanolgained water to increase the overall content to only 2.613%, while afterthe tenth run, the water content increased to only 2.779%. The averagecrystal size of each of these runs was only about 25 μm.

Thus, not only does the present procedure produce a unique crystal neverbefore realized in the sugar industry, but the procedure has reduced theenergy required to drive off solvent, and the crystallization medium isrecycled with a high degree of efficiency and reusability.

NON-ETHANOL EXAMPLES Acetone/Water

Another sample was run using acetone as the non-aqueoussugar-nondissolving liquid. Water was added to a content of 0.39%. To9.7 grams of the acetone/water above composition 0.1 gram of sucrosefloss was added. After only fifteen (15) minutes the uniquecrystallization of the present invention occurred. There was some rodcrystals resulting from the crystallization, but a significant amount ofspheroidal polycrystallite was also formed.

Benzene/Water

Another sample was run using benzene having a water content of about0.105%. The sugar floss was added to the benzene/water composition in anamount of about 5.0 grams. Again, the unique crystallization occurredbut at a rate somewhat slower than the ethanol/water composition.Basically, it took about three (3) weeks to obtain maximumcrystallization.

In order to provide a highly accelerated and efficient procedure, it ispresently believed that an anhydrous ethanol/water combination is themost preferred. The water should be included in the ethanol in an amountof not greater than 5%, preferably less than 3%, and most preferablyless than 2%. Floss should be added in an amount such that the floss toethanol ratio is not greater than 2 to 1 or not less than 1 to 120 byweight.

SURFACTANT EXAMPLES

Further experiments were conducted in which the surfactant lecithin wasused as part of the sugar feedstock which was processed to form theamorphous sugar. Specifically, 0.5% of lecithin was included in thesucrose feedstock. The material was processed using a high speedspinning apparatus at a temperature of about 160° C. and a spinningspeed of about 3600 rpm. The product resulting from the flash flowprocedure set forth above had the appearance of cotton candy.

The floss product resulting from the above procedure was then introducedto anhydrous ethanol which contained less than 1.0% water. A 1 gramsample of floss was immersed in 14 grams of the anhydrous ethanol/watercomposition at room temperature for a time period of about 2 minutes.The results indicated a highly uniform reduced-size polycrystallitespheroidal structure, which did not tend to aggregate. In fact, thepolycrystallites were on the order of about 4 μm. The tendency toaggregate is inherent in the growth of sugar crystals. The use of thesurfactant reduced the tendency to aggregate.

Moreover, the size range was smaller than that experienced with theprocedures using an amorphous sugar without a surfactant. Furthermore,the particle size was even more uniform than was the particle sizeresulting from the growth of polycrystallites which did not include asurfactant.

In conclusion, therefore, it is believed that the use of surfactant(especially lecithin) even further enhances the ability of the artisanto controllably grow uniform spheroidal polycrystallites having evensmaller dimensions than that experienced in the absence of thesurfactant. This capability provides the artisan with yet a further toolto engineer a product which is desired for use in sugar technology.

CRYSTALLITE EXAMPLES

In order to produce crystallites from the polycrystallite structuresprepared in accordance with the examples set forth above, water whichhad previously been essentially saturated was contacted with thespheroidal polycrystallite structures. In one case, saturated water wasprovided with an approximately 67% sucrose content. Water with 67%sucrose is essentially sugar saturated. As a result of contactingsaturated water solution with the polycrystallite product, thepolycrystallite disintegrated, dispersing the crystallites throughoutthe solution. The crystallites were made available for use in thesolution as a monodispersed crystallite product--to impart smoothfat-like mouthfeel.

Another experiment was conducted in which a polycrystallite product wasadded to 8.5% water. The polycrystallite structures were disintegratedreleasing the crystallites into the composition. FIG. 5a is aphotomicrograph taken at 450 magnification of the crystallites in acomposition which can be used as a fondant. In order to show theefficacy of this procedure and product, a photomicrograph taken at 450magnification of a fondant product prepared with fondant sugar known inthe art is shown in FIG. 5b. The comparison is dramatic. A fondantproduct prepared using crystallites of the present invention appears tohave a sandy consistency. The fondant prepared with the fondant sugarknown in the art has a gravel-like consistency. Clearly the sandyconsistency is much preferred for purposes of smoothness and flowabilityin a fondant composition.

FONDANT EXAMPLES

Examples of fondant cremes were prepared by addition of water to theunique polycrystallite sugar prepared in accordance with the presentinvention and compared to fondant cremes prepared from commercial sugarsupplied as Amerfond™ sugar from Amstar. Both fondant cremes wereprepared by using other fondant ingredients in accordance with the tableset forth below.

    ______________________________________                                        FONDANT TABLE                                                                             Inventive Fondant                                                                           Commercial Fondant                                  Ingredient  (Grams)       (Grams)                                             ______________________________________                                        Corn Syrup  14.00         14.00                                               Flavor, Raspberry                                                                         0.36          0.36                                                Citric Acid 0.80          0.80                                                Invertase   0.61          0.61                                                Color, Red (10%)                                                                          Trace         Trace                                               FDC # 40                                                                      ______________________________________                                         Water was added in order to achieve the correct viscosity for preparing       fondantcontaining confections, i.e., chocolate coated fondant candy.     

Surprisingly, it was found that the amount of inventive sugar requiredto obtain the correct viscosity was about 50% of the amount ofcommercial sugar required to achieve the same viscosity. In particular,it was found that only about 37 grams of the inventive sugar wasrequired to attain a viscosity of about 1.8 centipoises, whereas about67 grams by weight of the commercial sugar was required to attain thesame viscosity.

The compositions were prepared by dry mixing the ingredients and thenadding water while mixing. Water was added until the consistency of thecomposition attained a creamy smoothness. The fondant composition wasthen allowed to set before rolling and permitting to become firm.

As another interesting and unusual result, it was discovered that thecreme prepared with the inventive sugar required only fifteen (15)minutes of time to set to a firmness sufficient to handle, whereas thefondant creme prepared with the commercial sugar required thirty (30)minutes to set sufficiently for handling and dipping.

The cremes were then processed by dipping into chocolate. The cremesprepared with the sugar product of the present invention retained itsshape better while dipping. Moreover, immediately after the cremes wereproduced the inventive cremes had a smoother texture which was retainedover at least a five (5) day period.

The results of the fondant experiments were striking in that the amountof sugar required as well as the product itself were significantlyenhanced by use of the polycrystalline sugar of the present invention.

FAT MIMETIC EXAMPLES

Examples were also prepared in order to test the efficacy of thepolycrystallite sugar used in a confectionery filling which relies onfat as a medium for the organoleptic quality of the product. Inparticular, cookie fillings include fat in order to provide the texture,firmness, quality, and mouthfeel necessary to be used as a cookiefilling.

In order to test a cookie filling prepared with the present invention, aformulation was prepared which included a total of 84.94% sucrose. Inorder to prepare this composition, 35 grams of the polycrystallitespheroid product was combined with 29.4 grams of a saturated sucrosesolution. The saturated sucrose solution contained 30.59 grams ofsucrose and 15.06 grams of water, i.e., 67% sucrose.

4.8 gram samples were used to provide a filler between two Oreo™ cookiehalves. The cookies prepared in accordance with the present inventionwere tasted by a test panel. The results revealed that the cookiesprepared with the polycrystallite spheroid product of the presentinvention had a much cleaner mouthfeel, and were smoother and creamierthan the normal Oreo™ cookie filling. The commercial Oreo™ cookiefilling contains a great deal of fat. The composition of the presentinvention includes no fat.

Consequently, confectionery fillings for products can be prepared usingthe new crystals of the present invention and in order to eliminate orreplace fat in such fillings. Other and further uses will be apparent tothose skilled in the art and it is intended to include all such otheruses as come within the scope of the present invention.

CAKE ICING EXAMPLES

Further experiments were run to compare cake icings prepared with thespheroidal polycrystallite sugar of the present invention againstcommercial icings. Cake icing was prepared in accordance with theformulas set forth below in the table.

    ______________________________________                                        CAKE ICING                                                                                 Inventive Icing                                                                           Commercial Icing                                     Ingredient   (Grams)     (Grams)                                              ______________________________________                                        Commercial   --          227.0                                                Fondant Sugar                                                                 Inventive Sugar                                                                            227.0                                                            Corn Syrup,  9.0         9.0                                                  42 D.E.                                                                       Agar         1.18        1.18                                                 Simple Syrup 220.0       190.0                                                66 Brix. Soln.                                                                ______________________________________                                    

The sugars were placed in separate mixing vessels and blended with agar,after which the corn syrup was added. The simple sugar solutions werethen added until the desired consistency was achieved. As been notedbefore, the compositions prepared with the polycrystallite of thepresent invention required additional simple syrup because of thecapacity of the polycrystallite to include more water. The yield oficing was at least 7% greater using the polycrystallite sugar of thepresent invention. Thus, significantly less sugar is required when usingthe present invention.

The product using the polycrystallite spheroid sugar of the presentinvention was whiter, cleaner tasting, smoother texture, and had ahigher yield when compared to the commercial counterpart. It has beenfound that high quality fondant and fondant products can be producedwithout the requirement of making a fondant using conventional cooking,cooling and pulling equipment. Mere mixing in correct proportions hasbeen found to be adequate to prepare a high quality product using thepresent invention.

DONUT ICING EXAMPLES

The following example was an icing prepared for dipping baked goods orother comestibles in order to provide a coating. The present exampleswere used to provide a frosting for donuts.

The frosting was prepared in accordance with the formula set forth inthe table.

    ______________________________________                                        COATING FORMULATION                                                                      Inventive Coating                                                                          Commercial Coating                                    Ingredient (Grams)      (Grams)                                               ______________________________________                                        Commercial --           454                                                   Fondant Sugar                                                                 Inventive Sugar                                                                          454          --                                                    Corn Syrup 18           18                                                    42 D.E.                                                                       Water      76           60                                                    ______________________________________                                    

The ingredients were separately added while mixing hot water and drysugar. Afterward, corn syrup solids were added and additional water inorder to provide the correct consistency.

As can be seen, the sugar of the present invention required asignificant amount of additional water and resulted in a significantlylarger batch as a consequence. Thus, the coating prepared in accordancewith the present invention has a higher yield than does a coatingcomposition prepared with conventional fondant sugar.

Both coatings were used as icing for donuts by dipping the donuts intothe coating. The set time of the coating prepared in accordance with thepresent invention was much better. Specifically, the consistency of thecoating permitted easier immersion of a donut, and the coating set to afirmer and more appealing consistency, and adhered better to the donutsurface in a shorter period of time.

TABLET EXAMPLES

In order to show the efficacy of the present invention in variouscomestible forms, experiments were run to determine its usefulness intableting. In particular, 500 milligram samples of the spheroidalpolycrystalline sugar product was added to a tablet press and pressedunder 1.5 tons of pressure. Tablets were formed directly from thespheroidal polycrystallite product without the need for an additionalexcipient or, for that matter, any other tableting aid or vehicle.

The tablets formed were glossy and hard. However, when consumed, thehard tablets dissolved quickly in the oral cavity.

It appears that the polycrystallite product prepared in accordance withthe present invention can be tableted directly without the need for atableting aid. Moreover, tableting the new product does not require wetor dry granulation, or agglomeration. Thus, the spheroidalpolycrystallite product could be used directly to provide tablets or,indeed as an excipient for preparing other tablets with other materials.

The ready dissolution which occurs in the oral cavity is probablyattributable to the unique small polycrystallite structure. However, itis not intended that the present invention is in anyway limited by thehypotheses set forth herein.

Thus, while there had been described what are presently believed to bethe preferred embodiments of the present invention, those skilled in theart will appreciate that other and further modifications can be madewithout departing from the true scope of the invention, and it isintended to include all such modifications and changes as come withinthe scope of the claims as appended herein.

What is claimed is:
 1. A method of making a sugar productcomprising:controllably adding water to amorphous sugar formed byshearform processing in a non-aqueous sugar-nondissoluble liquid at atemperature wherein water is made available to said amorphous sugar at arate and in an amount which provides substantially spheroidalpolycrystallite structures.
 2. The method of claim 1 wherein saidstructures are monodispersed.
 3. The method of claim 1 wherein saidshearform process comprises subjecting said feedstock to shear createdby high speed spinning on a spinning head which casts materialoutwardly, said feedstock subjected to heating and shear in said headsufficient to create flash flow in said sugar carrier.
 4. The method ofclaim 1 wherein said shearform process comprises heating said feedstocksufficiently to provide internal flow in said sugar carrier, ejectingsaid feedstock while said sugar has said internal flow condition, andsubjecting said feedstock to disruptive fluid shear force to formmultiple masses of carrier.
 5. The method of claim 1 wherein saidamorphous sugar further comprises an additive whereby said additive isco-crystallized in said substantially spheroidal polycrystallitestructures.
 6. The method of claim 5 wherein said additive is a materialwhich can be integrated into said amorphous sugar without reducing theamorphism of said sugar and without deteriorating said substantiallyspheroidal polycrystallite structures.
 7. The method of claim 6 whereinsaid additive is selected from the group consisting of flavorants,bio-affecting agents, dyes, fragrances, food products, food ingredients,and other compatible agents.
 8. The method of claim 1 wherein said waterfurther comprises an additive which co-crystallizes with said sugar toform said substantially spheroidal polycrystallite structures.
 9. Themethod of claim 8 wherein said additive is selected from the groupconsisting of flavorants, bio-affecting agents, dyes, fragrances, foodproducts, food ingredients, and other compatible agents.
 10. The methodof claim 9 wherein said additive is a bio-affecting agent selected frominhalants.
 11. The method of claim 1 wherein said substantiallyspheroidal polycrystallite structures are microcrystalline.
 12. Themethod of claim 11 wherein the mean diameter of said polycrystallinestructures are not greater than about 50 μm.
 13. The method of claim 1wherein said non-aqueous sugar-nondissoluble liquid is maintained at atemperature of not less than about -20° C.
 14. The method of claim 1wherein said non-aqueous sugar-nondissoluble liquid and water form anazeotrope.
 15. The method of claim 14 wherein said water and said sugarnon-dissoluble liquid are combined in a azeotropic range.
 16. The methodof claim 14 wherein said non-aqueous sugar-nondissoluble liquid isethanol.
 17. The method of claim 1 wherein said water is present in anamount not greater than about 5% by weight.
 18. The method of claim 16wherein said water is present in an amount not greater than about 5.0%by weight.
 19. The method of claim 1 wherein said feedstock furthercomprises a surfactant.
 20. The method of claim 1 which furthercomprises disintegrating said spheroidal polycrystalline structures toform crystallites.
 21. The method of 20 wherein said disintegratingcomprises controllably adding an essentially sugar saturated aqueousliquid to said spheroidal polycrystallite structures.
 22. The method ofclaim 20 wherein said crystallites are not greater than withinmonodispersibility of 5 μm.
 23. A method of making a crystalline productcomprising:controllably adding a solvent to an amorphous solid form of asolvent-soluble compound, said solvent soluble compound capable offorming crystals, said controlled addition conducted in the presence ofa non-dissoluble liquid at a temperature and in an amount sufficient toform said crystalline product.
 24. The method of claim 23 wherein saidsolvent is water.